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Integration of two-dimensional (2D) nanometer-scale building blocks, such as graphene sheets, into 3D macroscopic structures (e.g., layered fi lms and porous scaffolds) is attracting much attention since it is an essential step in exploring the advanced properties of individual 2D sheets for practical applications. [ 1–32 ] For instance, freestanding graphene macroscopic structures have shown unique catalytic, electrochemical, and mechanical properties together with potential applications in chemical fi lters and electrodes for energy storage devices. [ 6–8 , 11 , 30 ] However, in most cases, during the process of assembling nanometerscale building blocks into macroscopic paper-like structures, the large accessible surface area of 2D graphene sheets is lost. The reason for this is that the individual graphene sheets tend to irreversibly aggregate and restack owing to the strong π - π stacking and van der Waals force between the planar basal planes of graphene sheets. This reduces the potential applications of graphene materials in electrochemical electrodes, composite materials, and so on. [ 20 ] Therefore, preventing aggregation of graphene sheets in the macroscopic structures, such that the properties of the individual graphene sheets are not compromised, is a critical challenge in constructing functional graphene-based macroscopic structures. Currently, a number of strategies for preventing aggregation have been developed, which include adding spacers (e.g., surfactants, nanoparticles, polymers), [ 27–36 ] template-assisted growth, [ 37 ] and crumpling the graphene sheets. [ 18 , 38 ] Alternatively, several groups have reported the formation of freestanding 3D graphene-based macroscopic structures without the assistance of any spacers or templates. [ 7 , 39,40 ] For instance, Li and coworkers reported the preparation of freestanding multilayered graphene fi lms by vacuum-assisted fi ltration based on the effective prevention of graphene intersheet restacking. [ 7 ] Shi and coworkers demonstrated the formation of a 3D graphene hydrogel by a hydrothermal method. [ 39 ] However, preparing freestanding and fl exible graphene fi lms with large accessible surface area but without complicated processing by overcoming the aggregation of graphene sheets remains a challenge